1. Field of the Invention
This invention relates to chemical reactions. In particular, the invention relates to the application of dynamic spin chemistry to electrolytic processes.
2. Description of Related Art
Since its discovery in 1944, Electron Spin Resonance (ESR) or Electron Paramagnetic Resonance (EPR), has been used to study chemical species having at least one unpaired electron. The combination of an applied DC magnetic field and electromagnetic radiation provides a resonant transition between two energy levels that allows for characterization of free radicals and their reactions.
In 1976-77, the Magnetic Isotope Effect (MIE) was discovered by Anatoly L. Buchachenko and others during investigation of the photolysis of dibenzyl ketone and benzoyl peroxide. In these particular cases, the MIE was due to a difference in spin evolution between radical pairs, depending upon whether the radical contained 13C or 12C. Nicholas J. Turro subsequently determined that the behavior of radical pairs could be modified by the use of micelles, thus enhancing the MIE.
Further research led by Buchachenko resulted in the discovery of the MIE for uranium in 1989. It has been shown that uranyl photoreduction by phenols is a spin-selective reaction. A uranium MIE has been determined in two uranyl photosensitized reactions: the oxidation of phenols and the decomposition of oxalic acid. Buchachenko and Khudyakov estimated a single stage separation factor of A=1.02 for the MIE, which exceeds their estimate of 1.006 for the classical mass isotope effect (CIE).
Buchachenko was involved in both the theoretical development (1981) of the Microwave Induced Magnetic Isotope Effect and its demonstration by the enhancement of MIE in dibenzyl ketone through microwave pumping in 1991. Microwave pumping has typically involved irradiation of a physically confined volume of solution. Since its discovery, application of the MIE has been focused on the use of micelles or other confinement techniques for radical pairs, and on the use of microwave radiation as a pumping source. Spin modification of chemical reactions through magnetic pumping may be applied to both magnetic and nonmagnetic compounds.
Aqueous electrolytes, aprotic solvents, room temperature ionic liquids (RTILs) and other fluids provide a wide base for the development of magnetically pumped electrolytic processes. For example, there are a limited number of volatile uranium compounds that may be used in laser, diffusion and centrifuge processes, but the combination of electrochemistry and dynamic spin chemistry offers a vast number of systems for the investigation of enhanced uranium enrichment and nuclear fuel reprocessing.
In general, the great variety and complexity of electrochemical systems precludes a comprehensive theoretical model of their behavior, and thus empirical methods must be relied on to a considerable extent. In the investigation of magnetic pumping of electrolytic reactions, it is desirable to have a compact inexpensive instrument for evaluating spin modification of electrochemical reactions so that research involvement is not limited by capital equipment requirements or space. For example, a tabletop system that can be constructed with readily available parts would minimize the barriers confronting potential investigators, allowing individuals of modest means to contribute to the development of the uranium enrichment and nuclear fuel reprocessing technologies.
In 2001, Buchachenko wrote “Besides the many factors controlling nuclear spin selectivity, there are two outstanding and highly promising but not yet properly exploited, microwave induced MIE and dimensionality.” Significantly, although the MIE for uranium and other elements has been established, an efficient approach to enhancement by microwave pumping has not been developed. Thus, there is a need for a system and method for providing efficient microwave pumping of unpaired electrons involved in chemical reactions. There is also a need for a compact, inexpensive, and scalable system that may be used in both research and manufacturing.